Research in the Waldie Group
Achieving a sustainable chemical future will require the development of efficient processes for the interconversion of electrical and chemical energy for renewable fuels production, fuel cell applications, and the synthesis of chemical feedstocks. The Waldie Group is interested in the rational design of molecular catalysts and supramolecular structures with targeted reactivity for these applications. We apply concepts from synthetic inorganic and organometallic chemistry coupled with electrochemical and spectroscopic techniques to prepare, understand, and optimize these systems and their reactivity.
Electro-Oxidation of Chemical Fuels
The electrochemical oxidation of fuels, such as H2, formic acid, and methanol, serves as the anodic half-reaction in fuel cells for electricity generation. Understanding how to promote these reactions through catalysis is critical to advance these technologies. We target molecular electrocatalysts that operate with high selectivity under mild conditions and offer precise active site control. Our efforts focus on earth abundant transition metal complexes with functional ligands to promote key proton & electron transfers.
Redox-Active Ligands as Electron Reservoirs
The redox activity of first-row transition metal ions is dominated by one-electron processes, but the introduction of redox-active ligands can be an effective strategy for achieving multielectron behavior. Our efforts focus on phenylenediamide complexes that exhibit a reversible two-electron oxidation. We use experimental & computational tools to study these systems, as well as to identify how their redox activity can be applied to promote small molecule activation via ligand-to-substrate electron transfer or hydrogen atom transfer.
Photochromic Framework Materials
Novel materials whose properties can be dynamically modulated when exposed to external stimulus are of great interest for smart responsive device technologies. Metal-organic frameworks (MOFs) offer an exciting versatile platform for constructing new light-responsive materials. We design and study new photochromic MOFs that incorporate light-responsive organic ligands into the network structure. We are especially interested in systems that exhibit optical control over the material electrical conductivity.